Kinetics of the Simplest Criegee Intermediate CH2OO Reaction with tert-Butylamine

Yang Chen; Haotian Jiang; Siyue Liu; Jiayu Shi; Yuqi Jin; Xueming Yang; Wenrui Dong

doi:10.1021/acs.jpca.2c07854

Kinetics of the Simplest Criegee Intermediate CH₂OO Reaction with tert-Butylamine

J Phys Chem A. 2023 Mar 23;127(11):2432-2439. doi: 10.1021/acs.jpca.2c07854. Epub 2023 Mar 13.

Authors

Yang Chen^{1

2

3}, Haotian Jiang^{3

4}, Siyue Liu^{3

5}, Jiayu Shi^{3

6}, Yuqi Jin^{2

3}, Xueming Yang^{3

7}, Wenrui Dong³

Affiliations

¹ Key Laboratory of Chemical Lasers, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
² University of Chinese Academy of Sciences, Beijing, 100049, China.
³ State Key Laboratory of Molecular Reaction Dynamics, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, China.
⁴ Department of Chemical Physics, School of Chemistry and Materials Science, University of Science and Technology of China, Hefei, 230026, China.
⁵ Key Laboratory of Materials Modification by Laser, Ion, and Electron Beams, Chinese Ministry of Education, School of Physics, Dalian University of Technology, Dalian, 116024, China.
⁶ Department of Physics, Dalian Maritime University, Dalian, Liaoning 116026, China.
⁷ Department of Chemistry, Southern University of Science and Technology, Shenzhen, 518055, China.

PMID: 36913641
DOI: 10.1021/acs.jpca.2c07854

Abstract

The kinetics of the simplest Criegee intermediate (CH₂OO) reaction with tert-butylamine ((CH₃)₃CNH₂) was studied under pseudo-first-order conditions with the OH laser-induced fluorescence (LIF) method at the temperature range of 283-318 K and the pressure range of 5-75 Torr. Our pressure-dependent measurement showed that at 5 Torr─the lowest pressure measured in the current experiment─this reaction was under the high-pressure limit condition. At 298 K, the reaction rate coefficient was measured to be (4.95 ± 0.64) × 10^-12 cm³ molecule^-1 s^-1. The title reaction was observed to be negative temperature-dependent; the activation energy of (-2.82 ± 0.37) kcal mol^-1 and the pre-exponential factor of (4.21 ± 0.55) × 10^-14 cm³ molecule^-1 s^-1 were derived from the Arrhenius equation. The rate coefficient of the title reaction is slightly larger than (4.3 ± 0.5) × 10^-12 cm³ molecule^-1 s^-1 of the CH₂OO reaction with methylamine; the electron inductive effect and the steric hindrance effect might play a role in contributing to such difference.